Uptake of Fe, Na and K atoms on low-temperature ice: implications for metal atom scavenging in the vicinity of polar mesospheric clouds.

1School of Environmental Sciences, University of East Anglia, Norwich, UK NR4 7TJ. bmurray@chem.ubc.ca

Abstract

Ice clouds form in the mesosphere between 80 and 90 km, at high latitudes during summer when the temperature falls below 150 K. There is strong evidence that the water-ice particles in these clouds scavenge metal atoms that are produced in the mesosphere by meteoric ablation. In the present study the uptake of Fe, Na and K on an ice film was studied in a fast flow tube over a temperature range of 80-150 K, covering the temperatures over which ice clouds form in the upper mesosphere. The uptake was found to be highly efficient and mostly in the diffusion-limited regime, requiring accurate measurements of the diffusion coefficients of the metal atoms in He: DFeHe = 366 (+/- 17) (T/296 K)(1.85 +/- 0.07), DNaHe 286 (+/- 13) (T/296 K)(1.68 +/- 0.04) and DKHe = 247 (+/- 15) (T/296 K)(1.69 +/- 0.07) Torr cm2 s(-1). Measured values of the diffusion coefficients in N2 are 112 (+/- 4), 125 (+/- 4) and 88 (+/- 4) Torr cm2 s(-1) at 293 K for Fe, Na and K, respectively. The uptake of Na and K was observed to be extremely efficient from 80-150 K, with lower limits of gamma Na > 0.09 and gamma K > 0.05, although it is likely that gamma is much closer to unity. The uptake of Fe on cubic ice is close to unity efficiency above 135 K, but gamma Fe decreases to only 3 x 10(-3) at 80 K. Uptake of Fe on amorphous ice films is much more efficient than on cubic ice films below 130 K. These results are interpreted using quantum calculations of the metal atoms adsorbed onto a 12-H2O model ice surface. Finally, it is shown that the uptake of Fe, Na and K on low-temperature ice is sufficiently fast to explain the substantial depletions in the mesospheric metal layers that are observed in the presence of mesospheric ice clouds.